Increasing the energy storage capability of lithium-ion batteries necessitates maximization of their areal capacity. This requires thick electrodes performing at near-theoretical specific capacity. However, achievable electrode thicknesses are restricted by mechanical instabilities, with high-thickness performance limited by the attainable electrode conductivity. Here we show that forming a segregated network composite of carbon nanotubes with a range of lithium storage materials (for example, silicon, graphite and metal oxide particles) suppresses mechanical instabilities by toughening the composite, allowing the fabrication of high-performance electrodes with thicknesses of up to 800 μm. Such composite electrodes display conductivities up to 1 × 104 S m−1 and low charge-transfer resistances, allowing fast charge-delivery and enabling near-theoretical specific capacities, even for thick electrodes. The combination of high thickness and specific capacity leads to areal capacities of up to 45 and 30 mAh cm−2 for anodes and cathodes, respectively. Combining optimized composite anodes and cathodes yields full cells with state-of-the-art areal capacities (29 mAh cm−2) and specific/volumetric energies (480 Wh kg−1 and 1,600 Wh l−1).
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The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.
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All authors acknowledge the SFI-funded AMBER research centre (SFI/12/RC/2278) and the Advanced Microscopy Laboratory for the provision of facilities and thank R. Charifou, who performed XRD for the samples. J.N.C. thanks Science Foundation Ireland (SFI, 11/PI/1087), the European Research Council (AdvGr FUTUREPRINT) and the Graphene Flagship (grant agreement no. 785219) for funding. V.N. thanks the European Research Council (SoG 3D2D Print) and Science Foundation Ireland (PIYRA) for funding.
The authors declare no competing interests.
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Supplementary Figs. 1–28, Supplementary Tables 8, Supplementary Note 1, Supplementary references